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Physical review. B, Condensed matter

Infrared spectral hole burning of sulfur-hydrogen deep donors in a Si: Ge crystal

S. P. Love, K. Muro, Robert E. Peale, Albert J. Sievers, W. Lo

Published Aug 15, 1987• 9 citations
Publisher

Abstract

Spectral holes which persist for \ensuremath{\sim}5 msec have been produced in the spectrum of a sulfur-hydrogen complex in a Si-0.1 at.% Ge alloy crystal maintained at 1.7 K. Measurements which combine an infrared laser pump with a Fourier-transform spectrometer probe show that the hole burning is due to migration of electrons from the S-H centers to shallow traps. The large observed hole width (4.6 ${\mathrm{cm}}^{\ensuremath{-}1}$) is attributed to spectral diffusion by resonant excitation transfer. The lack of temperature dependence of the hole burning of the $2{p}_{\ifmmode\pm\else\textpm\fi{}}$ line below 30 K suggests that excitation transfer is also responsible for the ionization of laser-excited centers in the hole-burning process.

DOI
10.1103/physrevb.36.2950

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Persistent spectral hole burning has been observed on the zero-phonon lines of the main site and several perturbed sites of ${\mathrm{Eu}}^{2+}$ in CaS:Eu single crystals. Hole burning occurs by two-step photoionization, can be strongly gated with IR irradiation, and takes place by excited-state absorption from the metastable ${4f}^{6}5d$ excited state to the conduction band followed by electron transport to ${\mathrm{Eu}}^{3+}$ centers which are the dominant traps. A complex hole structure consisting of a narrow feature (200 MHz), and broader features ($\ensuremath{\approx}5$ and $\ensuremath{\approx}100\mathrm{GHz}$) is observed. A mechanism is described for the occurrence of these unusually broad features. Time-varying internal electric fields which occur during the hole burning due to photoionization and trapping can lead to burning of holes at frequencies non-resonant with that of the laser. In addition, a mechanism for hole erasure, tunneling between Eu ions, is demonstrated. This mechanism is identified from the frequency dependence of the hole erasure which follows the ${\mathrm{Eu}}^{2+}$ absorption, and the linear dependence of the photoconductivity and hole erasure efficiency on irradiation power, both of which indicate erasure in a single-photon process.

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Persistent spectral hole burning (PSHB) and light-induced absorption spectra with the pump of burning light were measured and studied in the Sm2+-doped xAl2O3⋅(100−x)SiO2 glasses to reveal the electron transfer and the formation of PSHB at room temperature. It was observed that the density of Sm2+ at the burnt sites decreased, while that of Sm3+ increased after the burning. The hole depth increased with the increase of Al2O3 concentration. The formation of PSHB is attributed to a one-step electron transfer by tunneling through the excited state, D05. The traps that capture the electrons produced by the ionization of Sm2+ may be related to the oxygen vacancies. In addition, the thermal activated barrier height between the burnt and unburnt configuration was estimated as ∼1.0 eV by thermal hole filling.

Journal of Applied Physics•Nov 15, 1999•10 citations
Spectral holes which persist for \ensuremath{\sim}5 msec have been produced in the spectrum of a sulfur-hydrogen complex in a Si-0.1 at.% Ge alloy crystal maintained at 1.7 K. Measurements which combine an infrared laser pump with a Fourier-transform spectrometer probe show that the hole burning is due to migration of electrons from the S-H centers to shallow traps. The large observed hole width (4.6 cm\ensuremath−1{\mathrm{cm}}^{\ensuremath{-}1}cm\ensuremath−1) is attributed to spectral diffusion by resonant excitation transfer. The lack of temperature dependence of the hole burning of the 2p\ifmmode±\else\textpm\fi2{p}_{\ifmmode\pm\else\textpm\fi{}}2p\ifmmode±\else\textpm\fi​ line below 30 K suggests that excitation transfer is also responsible for the ionization of laser-excited centers in the hole-burning process.
In the first experimental search for persistent spectral hole burning in an elemental semiconductor, we examined a variety of electronic defects in Si and in a Si:Ge alloy. No persistent spectral changes have been observed for Be-Li, Se0, or thermal donors in Si; however, spectral holes which persist for ~5 ms have been produced in the 1s-2p absorption lines of a sulfur-hydrogen complex in Si. The addition of 0.7% Ge to the Si host ensures that an inhomogeneously broadened system is being studied. Measurements combining a CO2 laser pump with a Fourier transform spectrometer probe reveal that the hole burning is due to migration of electrons from the S-H centers to shallow traps. The large observed hole width (4.6 cm−1) is attributed to spectral diffusion by resonant excitation transfer. The hole burning behavior of the 2p± line is temperature independent below 30 K, whereas the hole burning of the 2p0 line exhibits strong temperature dependence, suggesting that the ionization of the laser-excited centers in the 2p± hole burning process occurs via energy transfer between neighboring excited centers rather than by thermal ionization.
With a ring dye laser persistent spectral hole-burning was measured by fluorescence excitation spectroscopy in the zero-phonon lines of the 2llg ↔ 2llu transition in KI:S2 − and of the 3H4 → 3P0 transition of a defect center with three D− ions in SrF2:Pr3+:D−and also in the zero-phonon line at 462.5 nm of a color center in neutron-irradiated and annealed α-Al2O3. In all three lines holes with a width in the order of 1 GHz could be obtained at 1.5 K with single frequency laser. With broad-band laser in KI:S2 − and SrF2:Pr3+:D− spectral redistribution within the full range of inhomogeneous broadening could be observed which are explained by a photophysical model based on barrier crossing in asymmetric double-well-potentials. In the case of sapphire a photobleaching process is dominant which is effective also for nonselective excitation, and the holes are thermoresistant up to 300 K.
Persistent spectral hole burning has been observed on the zero-phonon lines of the main site and several perturbed sites of Eu2+{\mathrm{Eu}}^{2+}Eu2+ in CaS:Eu single crystals. Hole burning occurs by two-step photoionization, can be strongly gated with IR irradiation, and takes place by excited-state absorption from the metastable 4f65d{4f}^{6}5d4f65d excited state to the conduction band followed by electron transport to Eu3+{\mathrm{Eu}}^{3+}Eu3+ centers which are the dominant traps. A complex hole structure consisting of a narrow feature (200 MHz), and broader features ($\ensuremath{\approx}5$ and $\ensuremath{\approx}100\mathrm{GHz}$) is observed. A mechanism is described for the occurrence of these unusually broad features. Time-varying internal electric fields which occur during the hole burning due to photoionization and trapping can lead to burning of holes at frequencies non-resonant with that of the laser. In addition, a mechanism for hole erasure, tunneling between Eu ions, is demonstrated. This mechanism is identified from the frequency dependence of the hole erasure which follows the Eu2+{\mathrm{Eu}}^{2+}Eu2+ absorption, and the linear dependence of the photoconductivity and hole erasure efficiency on irradiation power, both of which indicate erasure in a single-photon process.
Wavelength-selective excited-state lifetime measurements and absorption, luminescence, and hole-burning spectra of a natural African emerald crystal are reported. The (2)E excited-state lifetime displays an extreme wavelength dependence, varying from 190 to 37 μs within 1.8 nm of the R(1)-line. Overall, the excited state is strongly quenched, in comparison to laboratory-created emerald (τ=1.3 ms), with an average quenching rate of ∼6 × 10(3) s(-1) at 2.5 K. This quenching is attributed to photoinduced electron transfer caused by a relatively high concentration of Fe(2+) ions. The forward electron-transfer rate, k(f), from the nearest possible Fe(2+) sites at around 5 Å is estimated to be ∼20 × 10(3) s(-1) at 2.5 K. The photoreductive quenching of the excited Cr(3+) ions by Fe(2+) is followed by rapid electron back-transfer in the ground state upon deactivation. The exchange interaction based quenching can be modeled by assuming a random quencher distribution within the possible Fe(2+) sites with the forward electron-transfer rate, k(f), given as a function of acceptor-donor separation R by exp[(R(f)-R)/a(f)]; R(f) and a(f) values of 13.5 and 2.7 Å are obtained at 2.5 K. The electron transfer/back-transfer reorganizes the local crystal lattice, occasionally leading to a minor variation of the short-range structure around the Cr(3+) ions. This provides a mechanism for spectral hole-burning for which a moderately high quantum efficiency of about ∼0.005% is observed. Spectral holes are subject to spontaneous hole-filling and spectral diffusion, and both effects can be quantified within the standard two-level systems for non-photochemical hole-burning. Importantly, the absorbance increases on both sides of broad spectral holes, and isosbestic points are observed, in accord with the expected distribution of the "photoproduct" in a non-photochemical hole-burning process.
Persistent spectral hole burning (PSHB) and light-induced absorption spectra with the pump of burning light were measured and studied in the Sm2+-doped xAl2O3⋅(100−x)SiO2 glasses to reveal the electron transfer and the formation of PSHB at room temperature. It was observed that the density of Sm2+ at the burnt sites decreased, while that of Sm3+ increased after the burning. The hole depth increased with the increase of Al2O3 concentration. The formation of PSHB is attributed to a one-step electron transfer by tunneling through the excited state, D05. The traps that capture the electrons produced by the ionization of Sm2+ may be related to the oxygen vacancies. In addition, the thermal activated barrier height between the burnt and unburnt configuration was estimated as ∼1.0 eV by thermal hole filling.